3D Printing Self-Healing and Self-Adhesive Elastomers for Wearable Electronics in Amphibious Environments.

To meet the demands of challenging usage scenarios, there is an increasing need for flexible electronic skins that can operate properly not only in terrestrial environments but also extend to complex aquatic conditions. In this study, we develop an elastomer by incorporating dynamic urea bonds and hydrogen bonds into the polydimethylsiloxane backbone, which exhibits excellent autonomous self-healing and reversible adhesive performance in both dry and wet environments. A multifunctional flexible sensor with excellent sensing stability, amphibious self-healing capacity, and amphibious self-adhesive performance is fabricated through solvent-free 3D printing. The sensor has a high sensing sensitivity (GF = 45.1) and a low strain response threshold (0.25%) and can be used to detect small human movements and physiological activities, such as muscle movement, joint movement, respiration, and heartbeat. The wireless wearable sensing system assembled by coupling this device with a bluetooth transmission system is suitable for monitoring strenuous human movement in amphibious environments, such as playing basketball, cycling, running (terrestrial environments), and swimming (aquatic environments). The design strategy provides insights into enhancing the self-healing and self-adhesive properties of soft materials and promises a prospective avenue for fabricating flexible electronic skin that can work properly in amphibious environments.

[Determination of 10 carbamate pesticide residues in liquid milk by ultra performance liquid chromatography-tandem mass spectrometry with pass-through solid-phase extraction purification].

Carbamates are used in broad-spectrum insecticides and herbicides, and have highly efficient, low-residue, and long-lasting characteristics. However, this type of pesticide exerts mutagenic, teratogenic, carcinogenic, and other adverse effects, and its frequent use can exceed the recommended scope and limits. Research on the determination of carbamate pesticides mainly focuses on foods of plant origin and pays less attention to foods of animal origin. The methods for carbamate determination described in the current national standards have complicated operating procedures and low efficiency. Therefore, highly efficient and accurate methods for carbamate detection in milk must be established. In this work, a rapid method based on pass-through solid-phase extraction (SPE) purification coupled with ultra performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS) was developed for the simultaneous determination of 10 carbamate pesticides in liquid milk. The pretreatment and instrument methods were systematically optimized. The milk sample was extracted with acetonitrile, and then purified using a Captiva EMR-Lipid filtration kit. The purified extract was separated on an ACQUITY UPLC BEH C18 column with mobile phase of methanol and 0.1% formic acid aqueous solution in gradient elution. The flow rate was 0.3 mL/min. Column temperature was 35 ℃. Quantitative analysis was performed using the external standard method with matrix matching curves. The 10 carbamate pesticides showed good linear relationships in the mass concentration range of 2-200 µg/L, with correlation coefficients greater than 0.999. The limits of detection (LODs) and quantification (LOQs) for the 10 carbamate pesticides were 0.045-0.23 and 0.15-0.77 µg/kg, respectively. Recovery tests were conducted using the blank-matrix method at three spiked levels of 15, 50, and 100 µg/kg, and good recoveries for the 10 carbamate pesticides were obtained. In particular, the recoveries for the three spiked levels of 15, 50, and 100 µg/kg were 68.7%-93.3% with relative standard deviations (RSDs) of 1.8%-8.0%. The proposed method is efficient, convenient, accurate, and suitable for the rapid detection of the 10 carbamate pesticides in liquid milk. Compared with the conventional NH2 and ENVITM-18 SPE columns used in the national standard determination method, the proposed method demonstrated better purification effects. The recoveries for aldicarb sulfoxide, aldicarb sulfone, methomyl, and carbaryl after purification using the Captiva EMR-Lipid kit increased from 60% to 80%. Thus, the proposed method is suitable for targets with strong polarity and gives measurement results with good repeatability and accuracy.

Selective Laser Sintering of Polydimethylsiloxane Composites.

Conductive silicone elastomer carbon nanotubes (CNTs) composites possess potential applications in a variety of fields, including electronic skin, wearable electronics, and human motion detection. Based on a novel self-made covalent adaptable network (CANs) of polydimethylsiloxane (PDMS) containg dynamic steric-hindrance pyrazole urea bond (PDMS-CANs), CNTs wrapped PDMS-CANs (CNTs@PDMS-CANs) powders were prepared by a liquid phase adsorption and deposition, and were successfully used for selective laser sintering (SLS) three-dimensional printing. SLS-printed PDMS-CANs/CNTs nanocomposites possess high electrical conductivity and low percolation threshold as SLS is one kind of quasi-static processing, which leads to the formation of conductive segregated CNTs network by using the PDMS powders with special CNTs wrapped structure. The introduction of dynamic pyrazole urea bond endows the materials self-healing capability under electrothermal and photothermal stimulus. In addition, due to the resistance difference of the damaged and intact areas, crack diagnosing can be realized by infrared thermograph under electricity. In an application demonstration in strain sensor, the composite exhibits a regular cyclic electrical resistance change at cyclic compression and bending, indicating a relative high reliability.

Synthesis of a magnetic micelle molecularly imprinted polymers to selective adsorption of rutin from Sophora japonica.

Rutin is a naturally active compound with biological and medical value. The traditional extraction and separation method not only destroys the structure and activity of rutin, but results in a low extraction rate. In this work, the magnetic micellar molecularly imprinted polymer of rutin with a selective recognition function, i.e., RMMMIP was synthesized from 4 to Vinylphenylboron acid and 4-Vinylpyridine as functional monomer, derivatives of cholic acid as amphiphilic molecules. The internal hydrophobic and external hydrophilic characteristics of micelle was used to weaken the solvation of rutin and strengthen the non-covalent interaction between functional monomer and rutin. Fe3O4, as the core, endowed the composite materials with good magnetic responsiveness and was easy to separate solid from liquid. Then its structure and adsorption were studied, adsorbing capacity and recognition specific factor of RMMMIP are 11.9 mg·g-1 and 3.55 respectively. RMMMIP was used for the separation of rutin from crude extracts of Sophora japonica Linn and showed a better selective adsorption capacity than quercetin, naringin and cyanidin-3-O-glucose. It indicated that RMMMIP as a specific adsorbent had the potential to be a practical way to purify rutin from rutin crude extracts in the future.

Controllable construction of multifunctional superhydrophobic coating with ultra-stable efficiency for oily water treatment.

Designing interfacial coating with tailored characteristics is a crucial step in regulating the wetting properties of oil/water separation materials; however, the controllable fabrication of multifunctional layer with long-term durability in harsh environments remains challenging. Fabrication of raised dots based on magnetic Fe3O4 particles on micro-nanometer units, inspired by mussel chemistry, under the adhesion behavior of dopamine (DA) self-polymerization covalent deposition of Fe3O4 particles and hydrophobic polydimethylsiloxane (PDMS) modification to synthesize magnetic superhydrophobic cotton composites (Cotton-P). Due to the unique magnetic and superhydrophobic surface composition, the synthetic Cotton-P possesses superhydrophobic (155.4°) and magnetic properties and still exhibits these excellent properties after 10 cycles. In addition, the hydrophobicity of magnetic monolithic cotton is virtually unaffected in harsh environments. The chemical/thermal stability of the Cotton-P composite is improved due to the rigid silane coating on the skeleton. Moreover, the Cotton-P revealed excellent oil/water separation efficiency of over 98 % after 10 cycles. Based on these outstanding properties, Cotton-P has the potential to develop in the treatment of oil-water mixtures.

FSCN1 Promotes Glycolysis and Epithelial-Mesenchymal Transition in Prostate Cancer through a YAP/TAZ Signaling Pathway.

Objective: The aim of the study is to investigate the role and possible mechanism of fascin-1 (FSCN1) in the invasion, migration, glycolysis, and epithelial-mesenchymal transition (EMT) of prostate cancer. Methods: Real-time quantitative polymerase chain reaction (qRT-PCR) was utilized to determine the mRNA expression level of FSCN1 in prostate cancer tissues and prostate cancer cells PC-3 and DU145. The transwell and the scratch test were applied to detect the invasion and migration abilities of cells, respectively. A metabolic assay was used for measuring the glucose consumption, lactate production, and the extracellular acidification rate (ECAR) in cells; western blot was used for checking FSCN1, EMT, and yes-associated protein/transcriptional co-activators with the PDZ-binding motif (YAP/TAZ) signaling pathway-related protein expression level in cells or tissues. Results: FSCN1 was significantly highly expressed in prostate cancer tissues and cells. On the one hand, interference with the expression of FSCN1 could inhibit the invasion, migration, EMT, and glycolysis of prostate cancer cells. On the other hand, overexpression of FSCN1 promoted the invasion, migration, EMT, and glycolysis of prostate cancer cells. Besides, further mechanistic studies revealed that FSCN1 could activate the YAP/TAZ signaling pathway in prostate cancer cells. Conclusion: FSCN1 promotes invasion, migration, EMT, and glycolysis in prostate cancer cells by activating the YAP/TAZ signaling pathway. FSCN1 may be used as a biomarker for the diagnosis or treatment in prostate cancer.

Robust and recyclable graphene/chitosan composite aerogel microspheres for adsorption of oil pollutants from water.

Despite recent progress in graphene-based aerogels, challenges such as low mechanical strength and adsorption efficiency are still remaining. Here the reduced graphene oxide (rGO)/chitosan (CS) composite aerogel microspheres (rGCAMs) with center-diverging microchannel structures were developed by electrospraying and freeze-drying method. The optimized rGCAMs exhibit a high Young's modulus of 197 kPa and can support ~75,000 times its own weight, due to the cross-linking of CS by glutaraldehyde. Meanwhile, the rGCAMs can maintain high adsorption capacity for 15 cyclic tests due to its excellent mechanical strength. The oil adsorption kinetics and isotherms of rGCAMs follow the pseudo-second-order kinetic equation and the Langmuir model, respectively. The whole adsorption process is influenced by the oil diffusion in the liquid matrix and also in the intra-particle of aerogel microspheres. Moreover, rGCAMs can also be used to separate both surfactant-stabilized water-in-oil and oil-in-water emulsions through demulsification. The high-strength, recyclable and separation-efficient rGCAMs can be a potential candidate for oily wastewater treatment.

The Effect of the 3D Nanoarchitecture and Ni-Promotion on the Hydrogen Evolution Reaction in MoS2 /Reduced GO Aerogel Hybrid Microspheres Produced by a Simple One-Pot Electrospraying Procedure.

The transition toward renewable energy sources requires low-cost, efficient, and durable electrocatalysts for green H2 production. Herein, an easy and highly scalable method to prepare MoS2 nanoparticles embedded in 3D partially reduced (pr) graphene oxide (GO) aerogel microspheres (MoS2 /prGOAMs) with controlled morphology and composition is described. Given their peculiar center-diverging mesoporous structure, which allows easy access to the active sites and optimal mass transport, and their efficient electron transfer facilitated by the intimate contact between the MoS2 and the 3D connected highly conductive pr-GO sheets, these materials exhibit a remarkable electrocatalytic activity in the hydrogen evolution reaction (HER). Ni atoms, either as single Ni atoms or NiO aggregates are then introduced in the MoS2 /prGOAMs hybrids, to facilitate water dissociation, which is the slowest step in alkaline HER, producing a bifunctional catalyst. After optimization, Ni-promoted MoS2 /prGOAMs obtained at 500 °C reach a remarkable η10 (overpotential at 10 mA cm-2 ) of 160 mV in 1 m KOH and 174 mV in 0.5 m H2 SO4 . Moreover, after chronopotentiometry tests (15 h) at a current density of 10 mA cm-2 , the η10 value improves to 147 mV in alkaline conditions, indicating an exceptional stability.

Recent Advances of Self-Healing Polymer Materials via Supramolecular Forces for Biomedical Applications.

Noncovalent interactions can maintain the three-dimensional structures of biomacromolecules (e.g., polysaccharides and proteins) and control specific recognition in biological systems. Supramolecular chemistry was gradually developed as a result, and this led to design and application of self-healing materials. Self-healing materials have attracted attention in many fields, such as coatings, bionic materials, elastomers, and flexible electronic devices. Nevertheless, self-healing materials for biomedical applications have not been comprehensively summarized, even though many reports have been focused on specific areas. In this Review, we first introduce the different categories of supramolecular forces used in preparing self-healing materials and then describe biological applications developed in the last 5 years, including antibiofouling, smart drug/protein delivery, wound healing, electronic skin, cartilage lubrication protection, and tissue engineering scaffolds. Finally, the limitations of current biomedical applications are indicated, key design points are offered for new biological self-healing materials, and potential directions for biological applications are highlighted.

Biocompatible hypocrellin A-Fe(III) nanoparticles exhibiting efficient photo-activated CDT in vitro and in vivo.

Chemodynamic therapy (CDT) is novel and promising for cancer treatment, however, the potential systematic toxicity of the used nanoparticles is still a big concern. In this work the biocompatible hypocrellin A-Fe(III) nanoparticles (HA-Fe(III) NPs) were synthesized and studied. The CDT effect of HA-Fe(III) NPs in the dark is negligible but can be photo-activated upon red light irradiation, which is meaningful to realize precise CDT treatment by selective light irradiation. Moreover, HA-Fe(III) NPs can also generate O2˙-, which may be converted into H2O2 to further enhance the CDT effect. As a result, HA-Fe(III) NPs had little cytotoxicity in the dark at the concentration up to 200 µg ml-1, but exhibited efficient CDT activity upon red light irradiation under both normoxic and hypoxic conditions. The in vivo results also showed that HA-Fe(III) NPs can efficiently inhibit tumor growth upon 628 nm light irradiation.

An Alkynyl-Dangling Ru(II) Polypyridine Complex for Targeted Antimicrobial Photodynamic Therapy.

To realize clinical application of antibacterial photodynamic therapy (aPDT), one of the most arduous challenges is how to render aPDT agents high selectivity against bacterial pathogens. In light of the fact that amino group-containing lipids are rich on the outer surfaces of Gram-positive bacteria, we herein constructed an alkynyl-dangling ruthenium(II) polypyridine complex (Ru2) to preferentially label Staphylococcus aureus (S. aureus) and methicillin-resistant Staphylococcus aureus (MRSA) over mammalian cells via the amino-yne bio-orthogonal click reaction. Thanks to the strong singlet oxygen generation ability, Ru2 could photo-inactivate S. aureus and MRSA effectively and specifically. Phosphatidylethanolamine (PE) molecules also exist in mammalian cells but are not accessible for Ru2, leading to its poor binding/uptake and negligible cytotoxicity in the dark and upon irradiation towards mammalian cells as well as low hemolysis, all favorable for aPDT application.

Progress in Utilizing Dynamic Bonds to Fabricate Structurally Adaptive Self-Healing, Shape Memory, and Liquid Crystal Polymers.

Stimuli-responsive structurally dynamic polymers are capable of mimicking the biological systems to adapt themselves to the surrounding environmental changes and subsequently exhibiting a wide range of responses ranging from self-healing to complex shape-morphing. Dynamic self-healing polymers (SHPs), shape-memory polymers (SMPs), and liquid crystal elastomers (LCEs), which are three representative examples of stimuli-responsive structurally dynamic polymers, have been attracting broad and growing interest in recent years because of their potential applications in the fields of electronic skin, sensors, soft robots, artificial muscles, and so on. Recent advances and challenges in the developments toward dynamic SHPs, SMPs, and LCEs are reviewed, focusing on the chemistry strategies and the dynamic reaction mechanisms that enhance the performances of the materials including self-healing, reprocessing, and reprogramming. The different dynamic chemistries and their mechanisms on the enhanced functions of the materials are compared and discussed, where three summary tables are presented: A library of dynamic bonds and the resulting characteristics of the materials. Finally, a critical outline of the unresolved issues and future perspectives on the emerging developments is provided.

A Ru-anthraquinone dyad with triple functions of PACT, photoredox catalysis and PDT upon red light irradiation.

Phototherapy for cancer treatment has received much attention in recent years, and compounds with multiple anticancer mechanisms upon irradiation are particularly appealing. In this work, a nitro-anthraquinone group was attached to a biq (2,2'-biquinoline) ligand based Ru(ii) complex, endowing the resultant Ru1 compound with multiple anticancer mechanisms upon 600 nm light irradiation. Ru1 can undergo biq ligand photodissociation, showing its potential as a photoactivated chemotherapy (PACT) agent. Moreover, a Ru(iii) centre and an anthraquinone anion centre may be generated upon irradiation, which can further oxidize NADH/NADPH and generate O2˙-, successfully eliciting photoredox catalysis and photodynamic therapy (PDT). Compared to the control complex Ru2 without the nitroanthraquinone group, Ru1 exhibited much enhanced photocytotoxicity towards a series of cancer cell lines and 3D multicellular spheroids upon red light irradiation.

Comprehensive analysis of the functions and prognostic significance of RNA-binding proteins in bladder urothelial carcinoma.

Alterations in RNA-binding proteins (RBPs) are reported in various cancer types; however, the role of RBPs in bladder urothelial cancer (BLCA) remains unknown. This study aimed to systematically examine the function and prognostic significance of RBPs in bladder cancer using bioinformatics analyses. RNA sequencing and clinical data for BLCA were downloaded from The Cancer Genome Atlas (TCGA) database, and differentially expressed RBPs (DERBPs) between normal and cancer tissues were identified. A total of 388 DERBPs were identified, including 219 upregulated and 169 downregulated RBPs. All RBPs were screened for the prognostic model establishment and 9 RBPs (TRIM71, YTHDC1, DARS2, XPOT, ZNF106, FTO, IPO7, EFTUD2, and CTU1) were regarded as prognosis-related hub RBPs in BLCA. Further analysis revealed worse overall survival (OS) in the high-risk cohort compared to the model-based low-risk cohort. The area under the receiver operating characteristic (ROC) curve was 0.752 in the training group and 0.701 in the testing group, which supports the strength of its predictive ability. A nomogram was established according to nine prognosis-related RBPs, which showed strong predictive ability for BLCA. The C-indices of the nomogram were 0.7033 in the training group, and 0.6295 in the testing group. The prognosis-related hub RBPs may be involved in oncogenesis, development, and metastasis of BLCA. Our results will be of great significance in revealing the pathogenesis of BLCA, and developing new therapeutic targets and prognostic molecular markers for BLCA.

Hybrid Transition Metal Dichalcogenide/Graphene Microspheres for Hydrogen Evolution Reaction.

A peculiar 3D graphene-based architecture, i.e., partial reduced-Graphene Oxide Aerogel Microspheres (prGOAM), having a dandelion-like morphology with divergent microchannels to implement innovative electrocatalysts for the hydrogen evolution reaction (HER) is investigated in this paper. prGOAM was used as a scaffold to incorporate exfoliated transition metals dichalcogenide (TMDC) nanosheets, and the final hybrid materials have been tested for HER and photo-enhanced HER. The aim was to create a hybrid material where electronic contacts among the two pristine materials are established in a 3D architecture, which might increase the final HER activity while maintaining accessible the TMDC catalytic sites. The adopted bottom-up approach, based on combining electrospraying with freeze-casting techniques, successfully provides a route to prepare TMDC/prGOAM hybrid systems where the dandelion-like morphology is retained. Interestingly, the microspherical morphology is also maintained in the tested electrode and after the electrocatalytic experiments, as demonstrated by scanning electron microscopy images. Comparing the HER activity of the TMDC/prGOAM hybrid systems with that of TMDC/partially reduced-Graphene Oxide (prGO) and TMDC/Vulcan was evidenced in the role of the divergent microchannels present in the 3D architecture. HER photoelectron catalytic (PEC) tests have been carried out and demonstrated an interesting increase in HER performance.

High intensity focused ultrasound responsive release behavior of metallo-supramolecular block PPG-PEG copolymer micelles.

An amphiphilic metallo-supramolecular poly(propylene glycol)-block-poly(ethylene glycol) block copolymer containing a bis(2,2':6',2″-terpyridine) ruthenium (II) complex as a supramolecular connection between the two constituting blocks was used to prepare stable aqueous micelles which displayed a high intensity focused ultrasound (HIFU) triggered release behavior. By adjusting the HIFU time and intensity, the novel modality of HIFU triggered release allows for fine-tuning of the release kinetics of the encapsulants from the micelles in a remote and controlled way. Nuclear magnetic resonance spectroscopy, ultraviolet spectroscopy, and matrix-assisted laser desorption/ionization-time of flight mass spectrometry confirmed that the degradation of the micelles was due to the cleavage of the ether bond connected to the pyridine ring. This well controlled HIFU-copolymer micelle drug delivery system has considerable potential in targeted therapy.

Polyurethane-modified graphene oxide composite bilayer wound dressing with long-lasting antibacterial effect.

In order to obtain a novel multifunctional wound dressing with good water vapor permeability and long-lasting antibacterial properties, a skin-like thermoplastic polyurethane (TPU) bilayer membrane containing self-made polyhexamethylene guanidine hydrochloride (PHMG) grafted graphene oxide (MGO) was prepared by non-solvent phase separation and particle filtration. The antibacterial properties and wound-healing ability of TPU, GO-TPU, MGO-TPU composite porous membrane are systematically compared. The results show that with the incorporation of MGO, the porous MGO-TPU membrane exhibits good biocompatibility, excellent water vapor transmission properties, and long-lasting broad-spectrum antibacterial properties (the antibacterial property remains unchanged for 30 days under continuously shaking and washing). The wound healing results for mouse model show that MGO-TPU could significantly accelerate the healing rate of wounds as it provides a sterile environment and also promotes the formation of re-epithelialization during wound healing.

Constructing 3D Graphene Network in Rubber Nanocomposite via Liquid-Phase Redispersion and Self-Assembly.

A three-dimensional graphene (GE) segregated network structure is of significance for improving the conductivity of composites. However, constructing such a GE network structure in composites still remains a challenge. Here, we demonstrate a facile process, that is, liquid-phase redispersion and self-assembly (LRS) to prepare polymer nanocomposites with graphene segregated networks. High shear liquid-phase mixing accompanied by the diffusion of dissolved polymer chains into the interstices and voids of the loose graphene powders can lead to redispersion of GE in polymer solution. Once the stirring is stopped, the self-assembly and segregation of redispersed GE occurs in a poor solvent driven by π-π interaction. After solvent evaporation, the GE assembly structures are retained as networks in the GE/polymer composite prepared by hot pressing. The graphene/(isobutylene-isoprene rubber) nanocomposite (GE/IIR) was investigated as a demonstration for the advantages of the LSR method. The morphologies of GE assemblies in the liquid phase and GE networks in the solid composite were observed. Due to the existence of the homogeneously distributed graphene segregated networks, the tensile strength and elongation at break for GE/IIR nanocomposites increase by ∼410 and ∼126%, respectively, and the electrical conductivity reaches ∼100 S m-1 at a GE content of 3.76 vol %. The LRS method was also successfully tried for systems with different polymer matrixes and different solvents, suggesting the robustness of the proposed method. The prepared flexible GE/IIR nanocomposites with GE networks are sensitive to tiny strain and can be applied in wearable sensors for the detection of human physiological signals.

Novel Poly(vinyl alcohol)/Chitosan/Modified Graphene Oxide Biocomposite for Wound Dressing Application.

Rapid absorption of wound exudate and prevention of wound infection are prerequisites for wound dressing to accelerate wound healing. In this study, a novel kind of promising wound dressing is developed by incorporating polyhexamethylene guanidine (PHMG)-modified graphene oxide (mGO) into the poly(vinyl alcohol)/chitosan (PVA/CS) matrix, conferring the dressing the required mechanical properties, higher water vapor transmission rate (WVTR), less swelling time, improved antibacterial activity, and more cell proliferation compared to the PVA/CS film crosslinked by genipin. In vivo experiments indicate that the PVA/CS/mGO composite film can accelerate wound healing via enhancement of the re-epithelialization. PVA/CS/mGO composite film with 0.5 wt% mGO sheets displays the best wound healing properties, as manifested by the 50% higher antibacterial rate compared to GO and the wound healing rate of the mouse using this dressing is about 41% faster than the control group and 31% faster than the pure PVA/CS dressing. The underlying mechanism of the accelerated wound healing properties may be a result of the improved antibacterial ability to eradicate pathogenic bacteria on the wound area and maintain an appropriate moist aseptic wound healing environment to accelerate re-epithelialization. These findings suggest that this novel composite PVA/CS/mGO film may have promising applications in wound dressing.

4D Printing of a Liquid Crystal Elastomer with a Controllable Orientation Gradient.

Liquid crystal elastomers (LCEs), a class of soft materials capable of a large and reversible change in the shape under the trigger of external stimuli, can be fabricated into diverse architectures with complicated deformation modes through four-dimensional (4D) printing. However, the printable LCE ink is only in the form of monomeric precursors and the deformation mode is limited to contraction/extension deformation. Herein, we report a novel approach to break through these limitations. We achieved 4D printing of a single-component liquid crystal polymer ink in its isotropy state through direct ink writing (DIW) technology. The drawing force imposed by the movement of nozzle in the extruded printing process was able to align the mesogen units along the specific printing path. An orientation gradient perpendicular to the printing direction was obtained due to the existence of a temperature gradient between the two sides of printed samples and could be further fixed by post-photo-cross-linking treatment through the dimerizable groups in the LCE, realizing a new actuation mode in the field of extrusion-based printing of LCE actuators. The printed film was able to change reversibly from a strip to a tightly hollow cylinder and could reversibly lift up an object with roughly 600 times its own weight. The orientation gradient can be patterned through liquid-assistant printing or programmed structure design to integrate both bending and contraction actuation modes on the same printed sample, leading to complex deformation and two-dimensional (2D) planar porous structure to three-dimensional (3D) porous cylinder transition. This study opens up a new prospect to directly print a wide variety of LCE actuators with versatile actuation modes.